Characterization of ^{239,240}Pu Radionuclide Adsorption to Soil Particles and Mineral Dust Aerosols
Abstract
The release of ^{239,240}Pu into the environment by nuclear weapons testing 50 years ago initiated the cyclic mobilization of Pu-contaminated soil particles via the resuspension of dust resulting in a widespread distribution of Pu and other radionuclides. It is unclear what enables the aeolian transport of Pu in the environment; plausible hypotheses of Pu binding to dust and soil particles include Pu adsorption to iron oxides/hydroxides, organic acids, or silicate minerals such as clays. To investigate the connections between surface soils, dust and radionuclides, samples of soil and/or dust were collected from the Project Gnome Site in Eddy County, NM, the Jemez Mountains near Los Alamos, NM, and two 50-year old attics and wind-blown dust in Big Spring, TX. This study tests the hypothesis that Pu is adsorbed onto Fe oxides and hydroxides that coat dust/soil particles. The samples are generally low in organic carbon (0.2 - 4.8%, except for the unburned Los Alamos sample at 9.4%), as measured by LOI (Loss On Ignition) at 360 °C. The citrate-bicarbonate-dithionite method (CDB) of Fe oxide removal, first proposed by Mehra and Jackson in 1960, was used to selectively extract Fe oxides from the samples while leaving silicate Fe intact. Chemical digestion of each sample creates two fractions, the extracted supernatant and a solid pellet residue. If the Pu were associated with Fe oxides, then Fe and Pu should both be selectively removed from the bulk sample during the CBD process, leaving the pellet depleted in Fe and Pu and the supernatant enriched. For Fe, this was confirmed by scanning electron microscope and petrographic analyses. Preliminary radiochemical analyses of Pu activity also verify this hypothesis. Pu activity is significantly lower in pellets than bulk samples (Pu activitypellet/Pu activitybulk average = 0.07, range 0.02-0.12); Pu activity in supernatants is significantly higher than in bulk samples (Pu activitysupernatant/Pu activitybulk average = 4.45, range 2.53-6.92). The Big Springs wind-blown dust sample is an outlier; further analyses are in progress to evaluate its composition.
- Publication:
-
AGU Fall Meeting Abstracts
- Pub Date:
- December 2006
- Bibcode:
- 2006AGUFM.A53D0225T
- Keywords:
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- 0305 Aerosols and particles (0345;
- 4801;
- 4906);
- 0330 Geochemical cycles (1030);
- 1000 GEOCHEMISTRY;
- 1040 Radiogenic isotope geochemistry